KR20170055325A - Electrolyte layer for all-solid state battery and method of manufacturing the all-solid state battery using the same - Google Patents

Electrolyte layer for all-solid state battery and method of manufacturing the all-solid state battery using the same Download PDF

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KR20170055325A
KR20170055325A KR1020150158361A KR20150158361A KR20170055325A KR 20170055325 A KR20170055325 A KR 20170055325A KR 1020150158361 A KR1020150158361 A KR 1020150158361A KR 20150158361 A KR20150158361 A KR 20150158361A KR 20170055325 A KR20170055325 A KR 20170055325A
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electrolyte layer
electrolyte
slurry
layer
coating
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윤용섭
민홍석
김경수
권오민
신동욱
노성우
최락영
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현대자동차주식회사
한양대학교 산학협력단
기아자동차주식회사
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Priority to KR1020150158361A priority Critical patent/KR20170055325A/en
Priority to US15/181,569 priority patent/US10411294B2/en
Priority to CN201610509335.5A priority patent/CN106684464B/en
Priority to DE102016112378.1A priority patent/DE102016112378A1/en
Publication of KR20170055325A publication Critical patent/KR20170055325A/en

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    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
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Abstract

The present invention relates to a method for producing an all-solid battery. According to the present invention, the method for producing the all-solid battery comprises the following steps: forming a first electrolyte layer by coating first slurry on top of a base material with specific thickness; forming a second electrolyte layer by coating second slurry on top of the first electrolyte layer with specific thickness; bonding an electrode layer onto the second electrolyte layer through a pressing process after stacking the electrode layer on the second electrolyte layer; and detaching the base material from the first electrolyte layer. Additionally, since the first slurry on the first electrolyte layer contains less amount of a binder than the second slurry of the second electrolyte layer, the base material can be easily detached from the first electrolyte layer.

Description

전고체 배터리용 전해질층 및 이를 이용한 전고체 배터리의 제조방법{ELECTROLYTE LAYER FOR ALL-SOLID STATE BATTERY AND METHOD OF MANUFACTURING THE ALL-SOLID STATE BATTERY USING THE SAME}BACKGROUND OF THE INVENTION 1. Field of the Invention [0001] The present invention relates to an electrolyte layer for a solid-state battery, and a method for manufacturing an all-

본 발명은 전고체 배터리에 관한 것으로, 보다 상세하게는 전해질층과 전극층의 라미네이팅을 안정화시킴으로써 품질 확보가 유리한 전고체 배터리용 전해질층 및 이를 이용한 전고체 배터리의 제조방법에 관한 것이다. The present invention relates to an all solid-state battery, and more particularly, to an electrolyte layer for an all-solid-state battery in which quality assurance is secured by stabilizing lamination of an electrolyte layer and an electrode layer, and a method for manufacturing an all solid-state battery using the electrolyte layer.

널리 알려진 바와 같이, 전고체 전지(all-solid state battery)는 고분자 전해액을 고체 전해질로 대체함으로써 화학적 안정성을 도모함과 더불어, 누액이나 발화 등의 문제를 해결할 수 있다. As is widely known, an all-solid state battery can solve the problems of leakage, ignition, and the like, while achieving chemical stability by replacing the polymer electrolytic solution with a solid electrolyte.

이러한 전고체 전지는 고체전해질의 특성 향상 및 에너지밀도의 증가를 위하여 전극층 및 전해질층에 대한 후막화가 요구되고 있다. In order to improve the characteristics of the solid electrolyte and increase the energy density, such a solid electrolyte has been required to have a thicker electrode layer and an electrolyte layer.

이러한 전극층 및 전해질층의 후막화에 대응하기 위하여 전해질층과 전극층을 라미네이팅함으로써 전고체 배터리를 제조하는 방식이 이용되고 있다. In order to cope with the thickening of the electrode layer and the electrolyte layer, a method of manufacturing an all solid battery by laminating the electrolyte layer and the electrode layer has been used.

이러한 라미네이팅을 이용한 전고체 배터리의 제조방법을 구체적으로 살펴보면 다음과 같다. A manufacturing method of the all-solid-state battery using the laminating method will be described in detail as follows.

시트 또는 필름 등과 같은 기재(substarate) 위에 고체전해질 슬러리를 일정 두께로 코팅하여 건조시킴으로써 전해질층을 형성하고, 이에 전해질층의 일면에는 기재가 부착된 상태가 될 수 있다. A solid electrolyte slurry is coated on a substrate such as a sheet or a film to a predetermined thickness and dried to form an electrolyte layer, and a substrate may be attached to one surface of the electrolyte layer.

그리고, 전해질층의 타면에 양극 또는 음극의 전극층을 라미네이트(적층)한 후에 전해질층과 전극층을 프레스공정을 통해 접합한다. Then, an electrode layer of an anode or a cathode is laminated (laminated) on the other surface of the electrolyte layer, and then the electrolyte layer and the electrode layer are bonded through a pressing process.

그 이후에, 전해질층의 일면에 부착된 기재를 탈리(박리)하고, 전해질층의 일면에 반대극성의 전극층을 프레스 공정을 통해 접합할 수 있다. Thereafter, the substrate attached to one surface of the electrolyte layer is removed (peeled), and the electrode layer of the opposite polarity is bonded to one surface of the electrolyte layer through a pressing process.

하지만, 종래기술에 따른 전고체 배터리의 제조방법은 전해질층의 일면에서 원활하게 탈리되지 못하여 그 품질 확보가 불리하고, 또한 전해질층과 전극층 사이의 계면이 무너지는 단점이 있었다. However, the conventional method of manufacturing a solid-state battery according to the prior art has a drawback in that it can not be smoothly separated from one surface of the electrolyte layer, thereby deteriorating the quality thereof, and also disrupting the interface between the electrolyte layer and the electrode layer.

본 발명은 상기와 같은 종래기술의 단점을 해결하기 위하여 연구개발된 것으로, 서로 다른 바인더 함량을 가진 2층 이상의 전해질층을 구성함으로써 라미네이팅공법 적용 시에 전해질층로부터 기재의 탈리를 원활하게 함과 더불어, 전해질층과 전극층 사이의 계면을 원활하게 형성할 수 있는 전고체 배터리용 전해질층 및 이를 이용한 전고체 배터리의 제조방법을 제공하는 데 그 목적이 있다. Disclosure of Invention Technical Problem [8] Accordingly, the present invention has been made to overcome the above-mentioned disadvantages of the prior art, and it is an object of the present invention to provide an electrolyte layer having two or more layers having different binder contents, thereby facilitating the removal of the substrate from the electrolyte layer during the application of the laminating method An electrolyte layer for an all solid-state battery which can smoothly form an interface between an electrolyte layer and an electrode layer, and a method for manufacturing an all-solid-state battery using the same.

상기와 같은 목적을 달성하기 위한 본 발명의 일 측면은 전고체 배터리용 전해질층으로, According to an aspect of the present invention, there is provided an electrolyte layer for an all-solid-state battery,

2 이상의 전해질층이 적층되고, 상기 2 이상의 전해질층은 서로 다른 바인더 함량을 가지는 것을 특징으로 한다. Two or more electrolyte layers are stacked, and the two or more electrolyte layers have different binder contents.

상기 2 이상의 전해질층은 서로 다른 두께를 가지는 것을 특징으로 한다. The two or more electrolyte layers have different thicknesses.

상기 2 이상의 전해질층 각각은 바인더 및 용매가 혼합된 바인더 솔루션과, 고체 전해질을 가진 슬러리에 의해 형성되고, 상기 용매는 전해질과 반응성이 없는재질로 이루어지는 것을 특징으로 한다. Each of the two or more electrolyte layers is formed of a binder solution in which a binder and a solvent are mixed and a slurry having a solid electrolyte, and the solvent is made of a material which is not reactive with the electrolyte.

본 발명의 다른 측면은 전고체 배터리의 제조방법으로, Another aspect of the present invention is a method of manufacturing a pre-solid battery,

기재 위에 제1슬러리를 일정 두께로 코팅하여 제1전해질층을 형성하는 제1전해질층 형성단계;A first electrolyte layer forming step of forming a first electrolyte layer by coating a first slurry on a substrate to a predetermined thickness;

상기 제1전해질층 위에 제2슬러리를 일정 두께로 코팅하여 제2전해질층을 형성하는 제2전해질층 형성단계;A second electrolyte layer forming step of forming a second electrolyte layer by coating a second slurry on the first electrolyte layer to a predetermined thickness;

상기 제2전해질층에 전극층을 적층한 후에 프레스 공정을 통해 상기 제2전해질층에 전극층을 접합하는 접합단계; 및 A bonding step of bonding an electrode layer to the second electrolyte layer through a pressing process after laminating an electrode layer on the second electrolyte layer; And

상기 제1전해질층에서 기재를 탈리하는 기재 탈리단계;를 포함하고, And a base removing step of removing the base material from the first electrolyte layer,

상기 제1전해질층의 제1슬러리는 상기 제2전해질층의 제2슬러리 보다 바인더 함량이 적은 것을 특징으로 한다. Wherein the first slurry of the first electrolyte layer has a lower binder content than the second slurry of the second electrolyte layer.

상기 제1전해질층의 두께는 상기 제2전해질층의 두께 보다 작게 형성되는 것을 특징으로 한다. And the thickness of the first electrolyte layer is smaller than the thickness of the second electrolyte layer.

상기 제1전해질층 형성단계에서, 상기 제1슬러리의 코팅은 정전기 분무법에 의해 이루어지는 것을 특징으로 한다. In the first electrolyte layer forming step, the coating of the first slurry is performed by an electrostatic spraying method.

상기 제2전해질층 형성단계에서, 상기 제2슬러리의 코팅은 다이코팅(die coating), 콤마코팅(comma coating), 그라비아 코팅(Gravure coating) 중에서 어느 하나의 코팅공법에 의해 이루어지는 것을 특징으로 한다. In the second electrolyte layer forming step, the coating of the second slurry is performed by any one of coating methods such as die coating, comma coating and gravure coating.

상기 기재 탈리단계 이후에, 상기 제2전해질층에 접합되는 전극층과 반대극성을 가진 전극층을 상기 제1전해질층에 접합하는 것을 특징으로 한다. And an electrode layer having a polarity opposite to that of the electrode layer bonded to the second electrolyte layer is bonded to the first electrolyte layer after the substrate removing step.

이상과 같은 본 발명에 의하면, 서로 다른 바인더 함량을 가진 2 이상의 전해질층을 적층하는 구조로 전해질층을 구성함으로써 라미네이팅 공법 적용 시에 전해질층로부터 기재의 탈리를 원활하게 함과 더불어, 전해질층과 전극층 사이의 계면을 원활하게 형성할 수 있는 장점이 있다. According to the present invention, the electrolyte layer is formed by stacking two or more electrolyte layers having different binder contents, thereby facilitating the removal of the base material from the electrolyte layer during application of the laminating method, It is possible to form an interface smoothly.

도 1은 본 발명의 일 실시예에 따른 전고체 배터리의 제조방법을 도시한 공정도이다.
도 2는 본 발명에 의한 전고체 배터리의 제조방법에서 제1전해질층을 형성하는 과정을 도시한 도면이다.
도 3은 본 발명에 의한 전고체 배터리의 제조방법에서 제2전해질층을 형성하는 과정을 도시한 도면이다.
도 4는 본 발명에 의한 전고체 배터리의 제조방법에서 전해질층과 전극층을 적층하는 과정을 도시한 도면이다.
도 5는 본 발명에 의한 전고체 배터리의 제조방법에서 전해질층의 제2전해질층에 전극층을 접합하는 과정을 도시한 도면이다.
도 6은 본 발명에 의한 전고체 배터리의 제조방법에서 전해질층의 제1전해질층에서 기재를 탈리하는 과정을 도시한 도면이다.
도 7은 본 발명에 의한 전고체 배터리의 제조방법에서 전해질층의 제1전해질층에 전극층을 접합하는 과정을 도시한 도면이다. FIG. 1 is a process diagram illustrating a method of manufacturing an all solid state battery according to an embodiment of the present invention.
2 is a view illustrating a process of forming a first electrolyte layer in a method of manufacturing an all solid-state battery according to the present invention.
3 is a view illustrating a process of forming a second electrolyte layer in a method of manufacturing an all solid-state battery according to the present invention.
4 is a view illustrating a process of stacking an electrolyte layer and an electrode layer in a method of manufacturing an all solid-state battery according to the present invention.
5 is a view illustrating a process of bonding an electrode layer to a second electrolyte layer of an electrolyte layer in a method of manufacturing an all solid-state battery according to the present invention.
6 is a view illustrating a process of removing a substrate from a first electrolyte layer of an electrolyte layer in a method of manufacturing an all solid-state battery according to the present invention.
7 is a view illustrating a process of bonding an electrode layer to a first electrolyte layer of an electrolyte layer in a method of manufacturing an all solid-state battery according to the present invention.

이하, 본 발명의 바람직한 실시예를 첨부된 도면을 참조하여 상세히 설명한다. 참고로, 본 발명을 설명하는 데 참조하는 도면에 도시된 구성요소의 크기, 선의 두께 등은 이해의 편의상 다소 과장되게 표현되어 있을 수 있다. 또, 본 발명의 설명에 사용되는 용어들은 본 발명에서의 기능을 고려하여 정의한 것이므로 사용자, 운용자 의도, 관례 등에 따라 달라질 수 있다. 따라서, 이 용어에 대한 정의는 본 명세서의 전반에 걸친 내용을 토대로 내리는 것이 마땅하겠다.Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the accompanying drawings. For the sake of convenience, the size, line thickness, and the like of the components shown in the drawings referenced in the description of the present invention may be exaggerated somewhat. The terms used in the description of the present invention are defined in consideration of the functions of the present invention, and thus may be changed depending on the user, the intention of the operator, customs, and the like. Therefore, the definition of this term should be based on the contents of this specification as a whole.

도 1은 본 발명의 일 실시예에 따른 전고체 배터리의 제조방법을 도시한 공정도이다. FIG. 1 is a process diagram illustrating a method of manufacturing an all solid state battery according to an embodiment of the present invention.

도 1을 참조하면, 기재(10) 위에 제1전해질층(21)을 하는 제1전해질층 형성단계(S1)와, 제1전해질층(21) 위에 제2전해질층(22)을 형성하는 제2전해질층 형성단계(S2)와, 제2전해질층(22)에 전극층(31)을 적층하는 적층단계(S3)와, 제2전해질층(22)에 전극층(31)을 접합하는 제1접합단계(S4)와, 제1전해질층(21)에서 기재(10)를 탈리하는 기재 탈리단계(S5)와, 기재(10)가 탈리된 제1전해질층(21)에 반대극성의 전극층(32)을 접합하는 제2접합단계(S6)를 포함할 수 있다. 1, a first electrolyte layer forming step S1 of forming a first electrolyte layer 21 on a substrate 10 and a second electrolyte layer forming step 22 of forming a second electrolyte layer 22 on the first electrolyte layer 21 A first electrolyte layer forming step S2 for forming an electrode layer 31 on the first electrolyte layer 22; a laminating step S3 for laminating the electrode layer 31 on the second electrolyte layer 22; A base material tearing step S5 for removing the base material 10 from the first electrolyte layer 21 and a second electrode layer 32 having an opposite polarity to the first electrolyte layer 21 from which the base material 10 has been removed, And a second bonding step (S6) of joining the first and second substrates.

[제1전해질층 형성][Formation of first electrolyte layer]

도 2을 참조하면, 기재(10) 위에 제1슬러리를 일정 두께(t1)로 코팅한 후에 건조시킴으로써 제1전해질층(21)을 형성한다(S1). Referring to FIG. 2, the first slurry is coated on the substrate 10 with a predetermined thickness t1 and then dried to form the first electrolyte layer 21 (S1).

제1슬러리는 고체분말상태의 전해질과 제1바인더 솔루션을 포함하고, 제1바인더 솔루션은 바인더와 용매가 혼합되어 이루어질 수 있다. 이에, 제1전해질층(21)은 도 2와 같이 전해질 입자(21a)들이 바인더(21b)에 의해 결착되어 형성될 수 있다. The first slurry includes an electrolyte in a solid powder state and a first binder solution, and the first binder solution may be a mixture of a binder and a solvent. Thus, the first electrolyte layer 21 may be formed by binding the electrolyte particles 21a with the binder 21b as shown in FIG.

이와 같이, 기재(10) 위에 제1슬러리가 코팅된 이후에 건조되어 제1전해질층(21)이 형성됨에 따라, 제1전해질층(21)은 그 일면에 기재(10)가 부착된 상태가 된다. As the first slurry is coated on the substrate 10 and dried to form the first electrolyte layer 21, the first electrolyte layer 21 has a state that the substrate 10 is attached to one surface thereof do.

일 실시예에 따르면, 제1슬러리를 닥터블레이드를 이용하여 기재(10) 위에 0.5~30㎛의 일정 두께(t1)로 코팅한 후에, 수분 1ppm 이하의 분위기에서 90~130℃, 1~6시간 동안 건조함으로써 기재(10) 위에 제1전해질층(21)을 형성할 수 있다.According to one embodiment, the first slurry is coated on the substrate 10 with a doctor blade at a constant thickness (t1) of 0.5 to 30 占 퐉 and then dried at 90 to 130 占 폚 for 1 to 6 hours So that the first electrolyte layer 21 can be formed on the substrate 10.

한편, 용매는 전해질과 반응성이 없는 것으로 1.3cp@300K 이상의 점도를 가지는 재질로 이루어짐이 바람직하다. On the other hand, the solvent is preferably made of a material having a viscosity of 1.3 cp @ 300 K or more, which is not reactive with the electrolyte.

일 실시예에 따르면, 용매로는 Dodecane이 이용될 수 있으며, 바인더로는 poly(ethylene-co-propylene-co-5-methylene-2-norbornene)이 이용될 수 있다. According to one embodiment, Dodecane may be used as the solvent, and poly (ethylene-co-propylene-co-5-methylene-2-norbornene) may be used as the binder.

일 실시예에 따르면, 용매에 바인더를 0~2%의 무게비로 혼합하고, 그 혼합물을 sonication을 통하여 교반하면서 40℃로 가열시킴으로써 제1바인더 솔루션을 제조할 수 있다. 이와 같이, 제1바인더 솔루션은 종래기술에 따른 전고체 배터리의 전해질층 보다 낮은 바인더 함량을 가지고, 이를 통해 후술하는 기재(10)의 탈리를 보다 용이하게 할 수 있다. According to one embodiment, a first binder solution can be prepared by mixing the binder with a solvent in a weight ratio of 0 to 2% and heating the mixture to 40 캜 with stirring through sonication. Thus, the first binder solution has a lower binder content than the electrolyte layer of the prior solid-state battery according to the prior art, thereby making it easier to detach the substrate 10 described below.

그리고, 0~0.2wt%(O을 포함하지 않음)의 제1바인더 솔루션을 고체분말상태의 전해질에 첨가하여 혼합함으로써 50~70 wt%의 고형분을 가진 제1슬러리를 제조할 수 있다. Then, a first slurry having a solid content of 50 to 70 wt% can be prepared by adding and mixing a first binder solution of 0 to 0.2 wt% (not including O) to an electrolyte in a solid powder state.

그리고, 기재(10)는 Al, Ni 중에서 어느 하나의 재질로 이루어질 수 있다. The base material 10 may be made of any one of Al and Ni.

[제2전해질층 형성][Formation of Second Electrolyte Layer]

도 3을 참조하면, 제1전해질층(21) 위에 제2슬러리를 일정 두께(t2)로 균일하게 코팅한 후에 건조시킴으로써 제1전해질층(21)의 타면에 제2전해질층(22)을 형성한다(S2). 3, a second electrolyte layer 22 is formed on the other surface of the first electrolyte layer 21 by uniformly coating the second slurry with a predetermined thickness t2 on the first electrolyte layer 21, (S2).

제2슬러리는 고체분말상태의 전해질과 제2바인더 솔루션을 포함하고, 제2바인더 솔루션은 바인더와 용매가 혼합되어 이루어질 수 있다. 이에, 제2전해질층(22)은 도 3과 같이 전해질 입자(22a)들이 바인더(22b)에 의해 결착되어 형성될 수 있다. The second slurry includes a solid state powder electrolyte and a second binder solution, and the second binder solution may be a mixture of a binder and a solvent. The second electrolyte layer 22 may be formed by binding the electrolyte particles 22a with the binder 22b as shown in FIG.

이와 같이, 제1전해질층(21) 위에 제2슬러리가 코팅된 이후에 건조되어 제2전해질(22)이 형성됨에 따라, 제2전해질층(22)의 일면에는 제1전해질층(21)이 일체로 형성되어 있고, 제2전해질층(22)의 타면에는 후술하는 제1전극층(31)이 접합되는 접합면이 형성될 수 있다. The first electrolyte layer 21 is coated on the first electrolyte layer 21 and then dried to form the second electrolyte 22. A first electrolyte layer 21 is formed on one surface of the second electrolyte layer 22, And the other surface of the second electrolyte layer 22 may be formed with a bonding surface to which a first electrode layer 31 described below is bonded.

일 실시예에 따르면, 제2슬러리를 닥터블레이드를 이용하여 기재(10) 위에 50~80㎛의 일정 두께(t2)로 코팅한 후에, 수분 1ppm 이하의 분위기에서 90~130℃, 3~8시간 동안 건조함으로써 제1전해질층(21)의 타면에 제2전해질층(22)을 형성할 수 있다.According to one embodiment, the second slurry is coated on the base material 10 with a doctor blade at a constant thickness (t2) of 50 to 80 mu m, and then dried at 90 to 130 DEG C for 3 to 8 hours The second electrolyte layer 22 may be formed on the other surface of the first electrolyte layer 21.

한편, 용매는 전해질과 반응성이 없는 것으로 1.3cp@300K 이상의 점도를 가지는 재질로 이루어짐이 바람직하다. On the other hand, the solvent is preferably made of a material having a viscosity of 1.3 cp @ 300 K or more, which is not reactive with the electrolyte.

일 실시예에 따르면, 용매로는 Dodecane이 이용될 수 있으며, 바인더로는 poly(ethylene-co-propylene-co-5-methylene-2-norbornene)이 이용될 수 있다. According to one embodiment, Dodecane may be used as the solvent, and poly (ethylene-co-propylene-co-5-methylene-2-norbornene) may be used as the binder.

일 실시예에 따르면, 용매에 바인더를 2~10%의 무게비로 혼합하고, 그 혼합물을 sonication을 통하여 교반하면서 40℃로 가열시킴으로써 제2바인더 솔루션을 제조할 수 있다. 이와 같이, 제2바인더 솔루션은 종래기술에 따른 전고체 배터리의 전해질층과 유사한 바인더 함량을 가지고, 이를 통해 후술하는 전극층(31)과의 접합을 안정되고 견고하게 할 수 있다. According to one embodiment, a second binder solution may be prepared by mixing the binder with a solvent in a weight ratio of 2 to 10% and heating the mixture to 40 캜 with stirring through sonication. As such, the second binder solution has a binder content similar to that of the electrolyte layer of the prior solid-state battery according to the prior art, thereby making it possible to stabilize and bond the electrode layer 31 to be described later.

그리고, 0.5~3wt%의 제2바인더 솔루션을 고체분말상태의 전해질에 첨가하여 혼합함으로써 40~70 wt%의 고형분을 가진 제2슬러리를 제조할 수 있다. A second slurry having a solid content of 40 to 70 wt% can be prepared by adding 0.5 to 3 wt% of a second binder solution to an electrolyte in a solid powder state and mixing.

위로부터 알 수 있듯이, 제1전해질층(21)의 제1슬러리는 제2전해질층(22)의 제2슬러리 보다 그 바인더의 함량이 작게 형성될 수 있다. As can be seen from the above, the first slurry of the first electrolyte layer 21 may have a smaller content of the binder than the second slurry of the second electrolyte layer 22.

그리고, 제1전해질층(21)의 두께(t1)가 제2전해질층(22)의 두께(t2) 보다 작게 형성될 수 있다. 특히, 제1전해질층(21)의 두께(t1)는 후술하는 기재(10)의 탈리를 용이하게 함과 더불어 제2전해질층(22)과 접합력을 안정되게 유지할 수 있을 정도로 적절히 조절됨이 바람직할 것이다. The thickness t1 of the first electrolyte layer 21 may be smaller than the thickness t2 of the second electrolyte layer 22. [ In particular, it is preferable that the thickness t1 of the first electrolyte layer 21 is appropriately adjusted so as to facilitate separation of the substrate 10 to be described later and to stably maintain the bonding strength with the second electrolyte layer 22 will be.

[전해질층과 전극층의 적층단계][Stacking Step of Electrolyte Layer and Electrode Layer]

제1전해질층(21)의 일면에 제2전해질층(22)이 일체로 형성됨에 따라 도 4에 도시된 바와 같이, 제1전해질층(21)과 제2전해질층(22)이 적층되어 전해질층(20)을 구성할 수 있다. 그리고, 전해질층(20)의 제2전해질층(22)의 타면에 전극층(31)을 적층한다(S3). 여기서, 전극층(31)은 양극 또는 음극 중에서 어느 하나로 이루어질 수 있다. The second electrolyte layer 22 is integrally formed on one surface of the first electrolyte layer 21 so that the first electrolyte layer 21 and the second electrolyte layer 22 are laminated, Layer 20 can be constructed. Then, the electrode layer 31 is laminated on the other surface of the second electrolyte layer 22 of the electrolyte layer 20 (S3). Here, the electrode layer 31 may be formed of either a positive electrode or a negative electrode.

[제1접합단계][First bonding step]

이렇게 적층된 전해질층(20)과 전극층(31)을 5~20MPa 압력의 프레스공정을 통해 접합한다(S4). The stacked electrolyte layer 20 and the electrode layer 31 are bonded through a pressing process at a pressure of 5 to 20 MPa (S4).

[기재 탈리단계][Step of removing substrate]

전해질층(20)의 제2전해질층(22)에 전극층(31)이 접합된 상태에서, 도 6과 같이 기재(10)를 제1전해질층(21)의 일면에서 탈리한다(S5). The base material 10 is removed from one surface of the first electrolyte layer 21 as shown in FIG. 6 in a state where the electrode layer 31 is bonded to the second electrolyte layer 22 of the electrolyte layer 20 (S5).

[제2접합단계][Second Joining Step]

기재(10)가 탈리된 전해질층(20)의 제1전해질층(21)의 일면에 상술한 전극층(31)과 반대극성인 전극층(32)을 25~40MPa의 프레스공정을 통해 접합한다(S6). 예컨대, 제1접합단계(S5)에서 접합되는 전극층(31)이 양극인 경우에는 제2접합단계(S6)에서 접합되는 전극층(32)은 음극이 될 수 있고, 이와 달리 제1접합단계(S5)에서 접합되는 전극층(31)이 음극인 경우에는 제2접합단계(S6)에서 접합되는 전극층(32)은 양극이 될 수 있다. The electrode layer 32 of opposite polarity to the electrode layer 31 described above is bonded to one surface of the first electrolyte layer 21 of the electrolyte layer 20 from which the substrate 10 has been removed through a pressing process of 25 to 40 MPa ). For example, when the electrode layer 31 to be bonded in the first bonding step S5 is an anode, the electrode layer 32 to be bonded in the second bonding step S6 may be a negative electrode. Otherwise, the first bonding step S5 The electrode layer 32 to be bonded in the second bonding step S6 may be an anode when the electrode layer 31 is a cathode.

한편, 전극층(31, 32)은 전해질층(20)의 형성 전에 사전에 제조될 수도 있다. On the other hand, the electrode layers 31 and 32 may be prepared before the formation of the electrolyte layer 20.

일 실시예에 따르면, 전극층(31, 32)은 양극 복합체 또는 음극 복합체로 이루어질 수 있다. According to one embodiment, the electrode layers 31 and 32 may be made of a positive electrode composite or a negative electrode composite.

이러한 전극층(31, 32)의 제조과정을 구체적으로 살펴보면 다음과 같다. The manufacturing process of the electrode layers 31 and 32 will be described in detail as follows.

먼저, 양극 또는 음극 활물질(50~85wt%), 고체 전해질(35~15wt%), 도전재(2~5wt%)를 tube mixer, milling 등으로 1차적으로 혼합한다. First, the anode or anode active material (50 to 85 wt%), the solid electrolyte (35 to 15 wt%), and the conductive material (2 to 5 wt%) are primarily mixed by a tube mixer or milling.

그 이후에, 유발, non bubbling kneader, lanetary mixer, vortex mixer 중에서 어느 하나를 사용하여 2차적으로 혼합함으로써 전극 복합체를 형성한다. Thereafter, the electrode composite is formed by secondary mixing using any one of induced, non-bubbling kneader, lanetary mixer and vortex mixer.

이러한 전극 복합체에 바인더 솔루션(1~10wt%), 용매 등을 첨가하여 혼합함으로써 40~70 wt%의 고형분을 가진 슬러리를 형성한다. 이러한 슬러리를 닥터 블레이드를 이용하여 기재 위에 설정 두께(100~500㎛)로 코팅하고, 코팅된 양극 또는 음극 복합체를 90~130℃의 온도로 진공오븐에서 1~6h 동안 건조함으로써 양극 전극층 및 음극 전극층을 제조할 수 있다. 여기서, 기재는 Al, C-Al, Ni, Cu foil 중에서 어느 하나일 수 있다. A binder solution (1-10 wt%), a solvent, and the like are added to the electrode composite and mixed to form a slurry having a solid content of 40-70 wt%. The slurry was coated on the substrate with a doctor blade to a predetermined thickness (100 to 500 mu m), and the coated anode or anode composite was dried in a vacuum oven at a temperature of 90 to 130 DEG C for 1 to 6 hours, Can be prepared. Here, the substrate may be any one of Al, C-Al, Ni, and Cu foil.

한편, 제1전해질층(21)의 제1슬러리는 제2전해질층(22)의 제2슬러리에 비해 바인더 함량이 낮아 그 점도가 저하될 수 있으므로, 상술한 제1전해질층 형성단계(S1)에서는 제1전해질층(21)의 형성을 위한 제1슬러리의 코팅은 정전기 분무법(electrospray deposition)에 의해 이루어짐이 바람직할 수 있다. 이와 같이 정전기 분무법에 의해 제1슬러리의 코팅이 이루어짐에 따라 제1전해질층(21)의 두께(t1)를 균일하고 안정적으로 형성할 수 있다. Since the first slurry of the first electrolyte layer 21 has a lower binder content than that of the second slurry of the second electrolyte layer 22, the viscosity of the first slurry may be lowered. Therefore, in the first electrolyte layer forming step S1, The coating of the first slurry for forming the first electrolyte layer 21 may be preferably performed by electrospray deposition. As the first slurry is coated by the electrostatic spraying method as described above, the thickness t1 of the first electrolyte layer 21 can be uniformly and stably formed.

그리고, 제2전해질층(22)은 종래기술에 따른 전고체 배터리의 전해질층과 유사한 바인더 함량을 가지므로, 상술한 제2전해질층 형성단계(S2)에서는 제2전해질층(22)의 형성을 위한 제2슬러리의 코팅은 다이코팅(die coating), 콤마코팅(comma coating), 그라비아 코팅(Gravure coating) 중에서 어느 하나의 코팅공법에 의해 이루어질 수 있다. Since the second electrolyte layer 22 has a binder content similar to that of the electrolyte layer of the all-solid-state battery according to the prior art, the formation of the second electrolyte layer 22 in the second electrolyte layer forming step S2 The coating of the second slurry may be performed by any one of coating methods such as die coating, comma coating and gravure coating.

이와 같이, 본 발명은 제1슬러리의 바인더 함량이 제2슬러리의 바인더 함량 보다 낮음에 따라 제1전해질층(21)은 제2전해질층(22) 보다 낮은 접착성을 가질 수 있고, 이를 통해 제1전해질층(21)의 일면에 부착된 기재(10)를 탈리하는 것이 보다 용이해질 수 있고, 이를 통해 라미네이션 공정의 안전성을 확보할 수 있으므로 품질 확보가 매우 유리하다. As described above, according to the present invention, the binder content of the first slurry is lower than the binder content of the second slurry, so that the first electrolyte layer 21 can have adhesiveness lower than that of the second electrolyte layer 22, 1 It is easier to remove the base material 10 attached to one side of the electrolyte layer 21, thereby securing the safety of the lamination process.

그리고, 본 발명은 제1전해질층(21)과 제2전해질층(22)을 순차적으로 형성시켜 전해질층(20)을 구성함에 따라, 전해질층(20)의 두께를 균일하게 구현할 수 있고, 이를 통해 균일한 전류분포를 형성하여 배터리의 성능을 대폭 향상시킬 수 있다. The thickness of the electrolyte layer 20 can be uniformly realized by forming the electrolyte layer 20 by sequentially forming the first electrolyte layer 21 and the second electrolyte layer 22, And thus the performance of the battery can be greatly improved.

특히, 본 발명은 바인더의 함량이 상대적으로 낮은 제1전해질층(21)의 두께를 적절히 조절함으로써 전극층(31)과 전해질층(20) 사이의 계면 저항을 최소화할 수 있다. In particular, the present invention can minimize the interface resistance between the electrode layer 31 and the electrolyte layer 20 by appropriately adjusting the thickness of the first electrolyte layer 21 having a relatively low binder content.

이상, 본 발명의 구체적인 실시예를 설명하였으나, 본 발명은 이 명세서에 개시된 실시예 및 첨부된 도면에 의하여 한정되지 않으며 본 발명의 기술적 사상을 벗어나지 않는 범위 이내에서 당업자에 의하여 다양하게 변형될 수 있다.While the present invention has been described in connection with what is presently considered to be practical exemplary embodiments, it is to be understood that the invention is not limited to the disclosed embodiments, but, on the contrary, is intended to cover various modifications and equivalent arrangements included within the spirit and scope of the appended claims. .

10: 기재 20: 전해질층
21: 제1전해질층 22: 제2전해질층
31, 32: 전극층10: substrate 20: electrolyte layer
21: first electrolyte layer 22: second electrolyte layer
31, 32: electrode layer

Claims (8)

2 이상의 전해질층이 적층되고, 상기 2 이상의 전해질층은 서로 다른 바인더 함량을 가지는 것을 특징으로 하는 전고체 배터리용 전해질층.Wherein at least two electrolyte layers are stacked, and the two or more electrolyte layers have different binder contents. 청구항 1에 있어서,
상기 2 이상의 전해질층은 서로 다른 두께를 가지는 것을 특징으로 하는 전고체 배터리용 전해질층.The method according to claim 1,
Wherein the two or more electrolyte layers have different thicknesses. 청구항 1에 있어서,
상기 2 이상의 전해질층 각각은 바인더 및 용매가 혼합된 바인더 솔루션과, 고체 전해질을 가진 슬러리에 의해 형성되고, 상기 용매는 전해질과 반응성이 없는재질로 이루어지는 것을 특징으로 하는 전고체 배터리용 전해질층.The method according to claim 1,
Wherein each of the two or more electrolyte layers is formed of a binder solution in which a binder and a solvent are mixed and a slurry having a solid electrolyte, and the solvent is made of a material which is not reactive with the electrolyte. 기재 위에 제1슬러리를 일정 두께로 코팅하여 제1전해질층을 형성하는 제1전해질층 형성단계;
상기 제1전해질층 위에 제2슬러리를 일정 두께로 코팅하여 제2전해질층을 형성하는 제2전해질층 형성단계;
상기 제2전해질층에 전극층을 적층한 후에 프레스 공정을 통해 상기 제2전해질층에 전극층을 접합하는 접합단계; 및
상기 제1전해질층에서 기재를 탈리하는 기재 탈리단계;를 포함하고,
상기 제1전해질층의 제1슬러리는 상기 제2전해질층의 제2슬러리 보다 바인더 함량이 적은 것을 특징으로 하는 전고체 배터리의 제조방법.A first electrolyte layer forming step of forming a first electrolyte layer by coating a first slurry on a substrate to a predetermined thickness;
A second electrolyte layer forming step of forming a second electrolyte layer by coating a second slurry on the first electrolyte layer to a predetermined thickness;
A bonding step of bonding an electrode layer to the second electrolyte layer through a pressing process after laminating an electrode layer on the second electrolyte layer; And
And a base removing step of removing the base material from the first electrolyte layer,
Wherein the first slurry of the first electrolyte layer has a lower binder content than the second slurry of the second electrolyte layer. 청구항 4에 있어서,
상기 제1전해질층의 두께는 상기 제2전해질층의 두께 보다 작게 형성되는 것을 특징으로 하는 전고체 배터리의 제조방법.The method of claim 4,
Wherein the thickness of the first electrolyte layer is smaller than the thickness of the second electrolyte layer. 청구항 4에 있어서,
상기 제1전해질층 형성단계에서, 상기 제1슬러리의 코팅은 정전기 분무법에 의해 이루어지는 것을 특징으로 하는 전고체 배터리의 제조방법.The method of claim 4,
Wherein the coating of the first slurry is performed by an electrostatic spraying method in the first electrolyte layer forming step. 청구항 4에 있어서,
상기 제2전해질층 형성단계에서, 상기 제2슬러리의 코팅은 다이코팅(die coating), 콤마코팅(comma coating), 그라비아 코팅(Gravure coating) 중에서 어느 하나의 코팅공법에 의해 이루어지는 것을 특징으로 하는 전고체 배터리의 제조방법.The method of claim 4,
Characterized in that, in the second electrolyte layer forming step, the coating of the second slurry is performed by any one coating method of die coating, comma coating and gravure coating. A method of manufacturing a solid battery. 청구항 4에 있어서,
상기 기재 탈리단계 이후에, 상기 제2전해질층에 접합되는 전극층과 반대극성을 가진 전극층을 상기 제1전해질층에 접합하는 것을 특징으로 하는 전고체 배터리의 제조방법.
The method of claim 4,
Wherein an electrode layer having an opposite polarity to an electrode layer bonded to the second electrolyte layer is bonded to the first electrolyte layer after the base tear-off step.
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